Preparation Of Pd?Pt@MOFs And Research Of Catalysis Of Alcoholic Oxidation And Tandem Reaction

Nanotechnology has drawn extensive attention of experts and scholars since last century.With rapid development of science technology,nano-catalysis has already evolved into a new area.Because of their smaller size and larger specific surface area,metal nanoparticles have more catalytic activity sites.However,they usually tend to occur aggregation and difficult to be separated in practice.The traditional strategy is usually to load the nanoparticles on the carriers such as graphene,aluminum oxide,silicon dioxide,activated carbon.Although the activity of the loaded catalyst can be improved obviously,the catalysts are hard to recycle.Compared with traditional inorganic porous carriers,metal organic frameworks?MOFs?show greater advantages.Thiers coordinatively unsaturated metal centers and functional organic linkers make them excellent catalysts.Meanwhile,their tunable pore structure also makes them excellent carriers that confine nanoparticles to the holes exactly.So loading MNPs to the MOFs,not only effectively prevents MNPs from aggregating,improves catalytic activity,but also expands the application of MOFs.The novel MNPs@MOFs composite with good stability and recyclability is a excellent multifunction catalyst which has both MNPs and MOFs catalytic sites,and shows high activity to the catalyzed alcohol oxidation reactions and cascade reactions.The thesis consists four parts:The first part mainly introduced characteristics and applications of MOFs,synthesis methods and applications of MNPs@MOF,significance and content of research in this paper.The second part mainly introduced the synthesis and preparation methods of three kinds of porous MOFs materials including MIL-101,NH₂-MIL-101,UIO-66and four kinds of composite materials including Pd@MIL-101,Pd@NH₂-MIL-101,Pd@UIO-66,Pt@MIL-101.These properties of materials were characterized by the means of PXRD,IR,SEM,TEM,EDS,gas adsorption instrument.The third part mainly introduced the studies on the catalytic effects of MNPs@MOFs on alcohol oxidation and cascade reactions.The multifunction composite of Pd@MIL-101 can not only catalyze the oxidation of aromatic alcohols efficiently,but also catalyze the oxidation-amination cascade reactions.The multifunction composite of Pd@NH₂-MIL-101 showed high catalytic activity in the oxidation-Knoevenagel condensation cascade reactions.The fourth part was the conclusion part,which mainly summarized the synthesis methods and applications of the two kinds of composite materials of Pd@MIL-101and Pd@NH₂-MIL-101.They exhibited high catalytic activity and recyclability and potentials of applications in chemical industry.